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Soviet Journal of Quantum Electronics

Resonant four-photon parametric oscillation in the presence of a strong field due to a neighboring transition

G. M. Barykinsky, Vladimir V. Lebedev

Published Feb 28, 1981• 0 citations
Publisher

Abstract

An analysis is made of generation of the sum frequency ω3 = 2ω1 + ω2 in the case when the pump frequency coincides with that of a two-photon transition 2ω1 = ω21, and the frequency ω3 is tuned near the resonance line of an atom. Under conditions of resonance with the frequency of the generated field, the parametric process has some characteristic features associated with a strong competition between effects involving increases in the nonlinear susceptibility, absorption, and changes in the phase matching. Moreover, in the presence of a fairly high-intensity field due to a neighboring transition at the frequency ω2, a nonlinear Raman process (which changes the characteristics of the medium at the frequency ω3) begins to play an important part. It is found that the highest parametric oscillation powers over a wide spectral range may be achieved by appropriately varying the intensity of the field due to the neighboring transition, the atom concentration, or the interaction length.

DOI
10.1070/qe1981v011n02abeh005455

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An analysis is made of generation of the sum frequency ω3 = 2ω1 + ω2 in the case when the pump frequency coincides with that of a two-photon transition 2ω1 = ω21, and the frequency ω3 is tuned near the resonance line of an atom. Under conditions of resonance with the frequency of the generated field, the parametric process has some characteristic features associated with a strong competition between effects involving increases in the nonlinear susceptibility, absorption, and changes in the phase matching. Moreover, in the presence of a fairly high-intensity field due to a neighboring transition at the frequency ω2, a nonlinear Raman process (which changes the characteristics of the medium at the frequency ω3) begins to play an important part. It is found that the highest parametric oscillation powers over a wide spectral range may be achieved by appropriately varying the intensity of the field due to the neighboring transition, the atom concentration, or the interaction length.
An investigation was made of the spectral properties of four-photon parametric oscillation when the frequency of the generated field is tunable near an atomic resonance line. An ω4 = ω1–ω2+ω3 generation process involving coherent anti-Stokes scattering in thallium vapor was achieved experimentally. Biharmonic pumping was provided by resonant excitation of a 6P1/2–6P3/2 two-photon transition at the frequency ω1–ω2. Measurements were made of the oscillation power when the frequency ω3 was tunable near the frequency of a 6P3/2–7D3/2 transition at various thallium vapor pressures. It was found that the spectral properties of resonant parametric oscillation depend strongly on the concentration of active-mixture atoms and also on various saturation effects.
An investigation is reported of resonant four-wave frequency mixing of the type ω 4 =ω 1 —ω 2 +ω 3 under coherent population trapping conditions. Such mixing may appear when radiations of frequencies ω 1,2 are strong and when ω 1 —ω 2 =ω 20 (ω 20 is the frequency of a dipole-forbidden transition). The density matrix method is used to calculate (taking quantum interference into account) the absorption coefficients, the refractive indices, and the nonlinear susceptibilities exactly for the strong fields and in the first order of perturbation theory for the weak fields. A study is made of the dependence of the power of nonlinear optical generation on various characteristics of the transitions and of the radiation, subject to the propagation effects. The cases of homogeneous and Doppler broadening of the resonant transitions are considered. The characteristics of transitions in the barium atom are used in numerical illustrations. It is shown that the efficiency of resonant nonlinear-optical conversion of radiation can be enhanced by utilising interference processes in quantum transitions, which represent coherent population trapping.
We have considered the excitation spectra of three-photon processes arising from the interaction of a three-level atom, in the cascade configuration, with two strong electromagnetic fields whose initially populated modes ω a and ω b are near resonance with the atomic transition frequencies ω21 and ω32, respectively. In the limit of high photon densities, expressions for the Green's functions are derived in a closed form describing third order nonlinear processes in the region of frequencies ω = ω a + 2ω b and ω = ω b + 2ω a , respectively. Numerical calculations are then performed and the computed spectra are presented graphically for different values of the Rabi frequencies Ω a and Ω b , and detunings ζ a and ζ b , respectively. The excitation spectrum near ω = ω a + 2ω b is calculated as a function of the parameters η a = Ω a /γ0, η b = Ω b /γ0, ζ a = (ω21 - ω a )/γ0 and ζ b = (ω32 - ω b )/γ0 where γ0 is the spontaneous transition probability. With no detuning the spectral intensities vary slowly with respect to variations of the Rabi frequencies and are shifted by amounts governed by the field strengths η a and η b . In the presence of detunings, asymmetries, characteristics of such off-resonance situations, arise enhancing certain spectral peaks while diminishing the intensity of others.
It is shown that the resonance nonlinear susceptibility of four-photon parametric processes in gaseous media can be increased by several orders of magnitude. The increase in the susceptibility is due to suppression of the Doppler broadening of two-photon transitions in strong pump fields when the frequencies of the fields interacting with these transitions can be very different. Under these conditions there is an additional opportunity for increasing the susceptibility by reducing the frequency detuning relative to intermediate levels participating in two-photon transitions.
A theoretical analysis is made of the interaction between fields whose frequencies satisfy the relationship ωp–ωs=ωg±ωa≈ω21 , where ωp, ωs, ωg and ωa are the frequencies of the pump, Stokes, generated, and auxiliary fields; ω21 tne frequency of a transition between two levels in the investigated susbstance. The conditions are established for the maximum efficiency of the conversion of the fields ωp and ωa into the field ωg. It is shown that the optimal conversion conditions are obtained for a certain ratio of the pump and auxiliary field powers when the phases of the interacting waves are locked. Numerical estimates are obtained of the conversion efficiency and interaction length when the active substance is potassium vapor or compressed hydrogen.
We have considered the fluorescent spectra arising from the interaction of a four-level atom with two strong electromagnetic fields whose initially populated modes ω a and ω b are in resonance with three of the atomic transition frequencies. Green's function formalism has been used in the limit of high photon densities to calculate the excitation spectra near the frequencies ω = ±(2ω a - ω b ). Expressions for the total relative intensity of the system have been derived as a function of the parameter ζ = Ω2 b /Ω2 a , where Ω a and Ω b are the Rabi frequencies of the two laser fields, respectively. For ζ = 0, the spectra consist of a central peak at ω = 2ω a - ω b and a pair of sidebands at ω = 2ω a - ω b ± Ω a √2, both having spectral widths of the order of γ0, where γ0 is the spontaneous emission probability. The relative intensity of the central peak for Ω a ≠ 0 is reduced by 25 per cent of its original value obtained for Ω a = 0. For ζ ≠ 0, the relative intensity of the central peak increases slowly as ζ increases while that of the pair of sidebands at ω = 2ω b - ω b ± Ω a √2 is reduced by a factor of two of its given value for ζ = 0. This destructive interference is due entirely to the presence of the second laser field with Ω b ≠ 0. A new pair of sidebands, which arise from the cooperative effect of both laser fields, is peaked at ω = 2ω a - ω b ± Ω a √(2 + 0·5ζ) and has a spectral width equal to γ0. A set of four pairs of sidebands also appear at ω = 2ω a - ω b ± Cj (ζ)Ω a with j = 1, 2, 3, 4, respectively, which have spectral widths of the order of 3γ0/2. The existence of these pairs of sidebands depends strongly on the value of the parameter ζ. Numerical estimates for the coefficients Cj (ζ) and the relative intensities of these sidebands are tabulated for a wide range of values of ζ and discussed in detail.